We introduce a generalized approach to synthesize aerogels that allows remarkable control over its mechanical properties. The Hansen solubility parameters are used to predict and regulate the swelling properties of the precursor gels and, consequently, to achieve aerogels with tailored density and mechanical properties. As a demonstration, crosslinked organogels were synthesized from cellulose esters to generate aerogels. By determination of Hansen’s Relative Energy Difference, it was possible to overcome the limitations of current approaches that solely rely on the choice of precursor polymer concentration to achieve a set of aerogel properties. Hence, from a given concentration, aerogels were produced in a range of mass densities, from 25 to 113 mg/cm3. Consequently, it was possible to tailor the stiffness, toughness and compressive strength of the aerogels, in the ranges between 14–340, 4–103 and 22–373 kPa, respectively. Additionally, unidirectional freeze-drying introduced pore alignment in aerogels with honeycomb morphologies and anisotropy. Interestingly, when the swelling of the polymeric gel was arrested in a non-equilibrium state, it was possible to gain additional control of the property space. The proposed method is a novel and generic solution to achieving full control of aerogel development, which up to now has been an intractable challenge.